APPLIED SURFACE SCIENCE
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2022
·
IF 7.392
Hongjing Tian,Jin Du,Peng Lu,Shengnan Xu,Yanxia Guo,Jixing Tang,Man Wu,Qingjie Guo
A novel solid bi-amine adsorbent was synthesized by simultaneously impregnating pentaethylenehexamine (PEHA) and aminoethylethanolamine (AEEA) on the surfaces of mesoporous MCM–41 nanospheres. AEEA and PEHA had a synergistic effect during the CO 2 adsorption of the bi-amine adsorbent and the highest CO 2 adsorption capacity was 4.03 mmol·g −1 . The bi-amine adsorbent exhibited the favorable recyclability because its saturated CO 2 adsorption capacity decreased by 6.20 % after the initial eight adsorption/desorption cycles while by only 2.23 % in the following seven cycles. The adsorption activation energy and the desorption activation energy were determined to be 12.53 and 16.81 kJ·mol −1 , respectively. The low value of the desorption activation energy suggested an inconsiderable energy requirement in the multicycles of the adsorbent. The characterization results indicated that hydrogen bonds were formed between the hydrogen atom in hydroxyl groups of AEEA and the oxygen atom in carbonyl groups of the carbamate. The synergistic effect between AEEA and PEHA was unveiled on the CO 2 adsorption of the bi-amine adsorbent. The formed hydrogen bonds facilitated the release of protons from carbamic acids, enhanced the stability of the produced carbamate anions, and thus boosted the CO 2 adsorption performance.
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Journal of CO2 Utilization
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2022
·
IF 8.321
Fei Chen,Wensheng Wei,Yunsheng Gao,Yuxin Wang,Zizhen Yan,Zhanguo Zhang,Haiming Yu,Guangwen Xu,Lei Shi
Ionic liquid 1-ethyl-3-methylimidazolium ([Emim]IM) with high thermal stability and strong basicity was successfully synthesized. Using [Emim]IM as catalyst, dimethyl carbonate (DMC) was directly synthesized from epoxy propane (PO), CO 2 , and methanol under mild reaction conditions. A continuous two-stage DMC synthesis process was developed. The cycloaddition of CO 2 and PO was first conducted to produce propylene carbonate (PC), and then methanol was introduced into the system to synthesize DMC. During the cycloaddition process, 97.40% PO conversion and 97.40% PC yield were achieved with TON of 99.49. In the subsequent transesterification stage, DMC yield attained 83.63% with selectivity higher than 99% and TON of 70.15. [Emim]IM was reused for seven times without obvious deactivation, exhibiting good stability. The effects of reaction temperature, reaction time, the initial pressure of CO 2 , and catalyst weight on cycloaddition and transesterification reactions were systematically investigated. The kinetic study showed that the activation energies (E a ) of cycloaddition and transesterification reactions were 28.02 and 38.53 KJ·mol −1 , respectively, much lower than those of catalysts reported in the literatures. In addition, [Emim]IM displayed superior catalytic activity for the cycloaddition of CO 2 with various epoxy compounds .
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Electrocatalysis
·
2022
·Vol. 14
·期 1
·29-38
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IF 2.933
Fang Yu,Yu Yu,Zhao Wei,Yang Pengxin,Huang Tao,Gao Shan
Electrocatalytic CO 2 conversion to value-added chemicals is a fascinating strategy for the sustainable recycling of greenhouse gas while developing a facile synthesis method for highly efficient electrocatalysts remains a great challenge. Herein, the spontaneous alkali corrosion combined with in situ electrochemical restructuring strategy was developed to fabricate the self-supporting Zn nanosheets array (Zn NSs) on Zn foil for CO 2 electroreduction. The in situ transformed two-dimensional Zn NSs provide larger active area and show faster reaction kinetics and electron transfer rate compared with Zn nanoparticles and Zn foil, thus exhibiting outstanding performance for electrocatalytic CO 2 to CO: j CO is 9.9 mA cm −2 and 19.8 mA cm −2 at −0.9 and −1.0 V vs. RHE, respectively; Faraday efficiency (FE) of CO reaches 92% at −0.9 V vs. RHE; the stability can remain 14 h at −0.9 V vs. RHE. This work provides a facile and low-energy-consumption method to fabricate efficient electrocatalysts for CO 2 recycling. Graphical Abstract The present work presents simple spontaneous corrosion and in situ electrochemical restructuring strategy to get Zn nanosheets for electrocatalytic reduction of carbon dioxide, featuring its synthetic strategy and electrocatalytic CO 2 reduction performance.
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ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Zhiyan Si,Linkai Wang,Yu Han,Jiafeng Yu,Qingjie Ge,Chunyang Zeng,Jian Sun
Catalytic hydrogenation of carbon dioxide into chemicals and fuels has moved into the spotlight in the recent carbon-neutral age. However, this sustainable process is still a low efficiency one due to the limitations of the catalyst materials. Herein, we designed a highly active CuNaFe catalyst with a self-made physical sputtering method for CO2 hydrogenation. The total space time yield (STY) rate of high-value olefin and ethanol can reach as high as 833 mg·g–1·h–1 under a mild condition of 310 °C and 3 MPa, which ranks as one of the top performances among related studies. The characterizations demonstrate that the surface of highly dispersed Cu nanoparticles coupled with surrounding Na modified Fe5C2 creates a well-matched process of C–O activation, C–C coupling, and C–O insertion. These findings provide a new and general strategy to fabricate a high-efficiency catalyst for direct CO2 hydrogenation into useful chemicals.
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APPLIED ENERGY
·
2022
·
IF 11.446
Boshu Jiang,Bachirou Guene Lougou,Hao Zhang,Boxi Geng,Lianxuan Wu,Yong Shuai
The solar-driven thermochemical CO 2 -to-CO conversion is an effective way to achieve the mission of carbon peaking and carbon neutrality. However, synthesizing porous reacting materials with excellent thermal stability, hardness and long-term cyclic stability, oxygen exchange capacity, and higher CO 2 -to-CO conversion are the most important challenges associated with the thermochemical CO 2 -splitting approach and technological upscaling to large-scale applications. This study presented the development of NiFe 2 O 4 oxygen carriers, the synthesis method of SiC and Si 3 N 4 supports, and solar-to-fuel processing of the newly prepared materials through CO 2 -splitting under a highly concentrated solar radiative heat flux. The newly synthesized NiFe 2 O 4 @SiC porous redox material resulted in higher solar energy absorption and CO 2 conversion capability with an instantaneous CO production of 410 μmol/g and direct CO 2 -to-CO conversion rate of 18.1 % at 1073–1273 K reaction temperature. The media composite of NiFe 2 O 4 @SiC exhibited high-temperature thermal changes, good thermochemical reaction stability, and a higher CO production rate through six redox cycles compared to NiFe 2 O 4 @Si 3 N 4 porous reacting material. The high oxidation potential and remarkably solar radiative heat flux absorption and thermochemical CO 2 -splitting capacities of the newly developed materials were demonstrated through experimental analysis. The synergistic effect of the oxygen carriers (NiFe 2 O 4 ) and substrate materials including SiC and Si 3 N 4 skeletons for CO 2 -splitting is highlighted. This study provided comprehensive and novel experimental insights that can be used as guidance for theoretical research and application in CO 2 conversion into high-value-added energy products.
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Journal of Environmental Chemical Engineering
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2022
·
IF 7.968
Pan Ma,Meili Ding,Wei Rong,Xi Liu,Jianfeng Yao
The synergistic catalysis involving multiple active sites provides a promising method for improved catalytic activity . In this work, we developed a gentle acetic acid-assisted polyhydroxy acid modification strategy to regulate the coordination environment of a zirconium-based MOF , UiO-66. D -gluconic acid with multiple hydroxyl groups is selected to replace the acetic acid coordinated at the metal nodes of UiO-66 via competitive coordination, allowing for the coexistence of hydrogen bonding donors and Lewis acid sites. The effect of acetic acid and D -gluconic acid separately as modulator and modifier agent to produce linker defects on catalytic properties of UiO-66 was investigated in the cycloaddition of carbon dioxide (CO 2 ) with epichlorohydrin. It was demonstrated that the activity of UiO-66 can be tuned by the amount of D -gluconic acid. Remarkably, the resultant UiO-66-GA-1200, which is modified with 1200 μL of D -gluconic acid, achieves a high catalytic yield for CO 2 cycloaddition of epichlorohydrin under 1 bar CO 2 and 60 °C. In contrast of pure UiO-66, UiO-66-GA-1200 shows admirable catalytic activities (92–94% yield) even after exposure to humid environment or in simulated flue gas . This work provides a novel method for constructing MOF-based solid acid catalysts and casts a new light on the development of practical CO 2 utilization.
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JOURNAL OF CATALYSIS
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2022
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IF 8.047
Wenhao Li,De-Kun Ma,Xia Hu,Faliang Gou,Xiaogang Yang,Walker MacSwain,ChenZe Qi,Weiwei Zheng
Rationally designing and controlling the interactions between reaction intermediates and the surface of photocatalysts is critical to obtain high product selectivity in photocatalysis. Herein, using CdS-based photocatalytic CO 2 reduction reaction (CO 2 RR) as a model system, we demonstrate that CH 4 selectivity can be significantly enhanced through the introduction of La 3+ ions with high oxophilicity on the surface of the photocatalysts. The high surface oxophilicity of the photocatalysts can increase CO* desorption energy and promote further hydrogenation to CH 4 . In contrast, when Au 3+ ions with low oxophilicity were doped in CdS, reduced CH 4 selectivity was observed in the CO 2 RR. Significantly, enhanced CH 4 selectivity can be achieved by doping oxophilic La 3+ ions into a broad range of alternative photocatalysts including ZnO, SnS 2 , BiOBr, BiVO 4 , TaON, and CsPbBr 3 , which demonstrates the general strategy to enhance CH 4 selectivity of photocatalytic CO 2 RR through increased surface oxophilicity of the photocatalysts by rare earth La 3+ ion doping.
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Catalysis Science & Technology
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2022
·Vol. 12
·期 23
·7057-7064
·
IF 6.177
Lin Cheng,Changchang Wu,Huifang Feng,Hong Liu
2D MOFs show great potential in photocatalysis owing to their ultrathin thickness, large surface area and highly accessible active sites. Nevertheless, studies applying 2D MOFs as photocatalysts are very limited, especially for photocatalytic CO2 reduction. In this paper, a novel 2D/2D Co-PMOF/GR heterojunction was successfully constructed by coupling a 2D cobalt porphyrin-based MOF (Co-PMOF) and graphene (GR). The resultant Co-PMOF/GR composites could efficiently reduce CO2 to CO and CH4 under visible-light illumination without any assistance of a sacrificial agent and photosensitizer. When the content of GR was 10 wt%, the Co-PMOF/GR composite presented an optimum catalytic performance. The maximum yields of CO and CH4 over the Co-PMOF/GR composite reached 20.25 and 1.61 μmol g−1 h−1, respectively, which were 2.84 and 2.44 times those over pristine Co-PMOF. The enhanced catalytic efficiency was due to the synergy of higher light harvesting, enhanced CO2 absorption and efficient charge migration within the conductive and intimate 2D heterostructure. This study offers a new idea for the fabrication of highly active 2D MOF-based photocatalysts for solar energy conversion.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-10
·
IF 17.694
Wang Qiyou,Liu Kang,Hu Kangman,Cai Chao,Li Huangjingwei,Li Hongmei,Herran Matias,Lu Ying-Rui,Chan Ting-Shan,Ma Chao,Fu Junwei,Zhang Shiguo,Liang Ying,Cortés Emiliano,Liu Min
Atomically dispersed transition metals on carbon-based aromatic substrates are an emerging class of electrocatalysts for the electroreduction of CO 2 . However, electron delocalization of the metal site with the carbon support via d-π conjugation strongly hinders CO 2 activation at the active metal centers. Herein, we introduce a strategy to attenuate the d-π conjugation at single Ni atomic sites by functionalizing the support with cyano moieties. In situ attenuated total reflection infrared spectroscopy and theoretical calculations demonstrate that this strategy increases the electron density around the metal centers and facilitates CO 2 activation. As a result, for the electroreduction of CO 2 to CO in aqueous KHCO 3 electrolyte, the cyano-modified catalyst exhibits a turnover frequency of ~22,000 per hour at −1.178 V versus the reversible hydrogen electrode (RHE) and maintains a Faradaic efficiency (FE) above 90% even with a CO 2 concentration of only 30% in an H-type cell. In a flow cell under pure CO 2 at −0.93 V versus RHE the cyano-modified catalyst enables a current density of −300 mA/cm 2 with a FE above 90%.
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PubMed
高影响因子
Chemistry-An Asian Journal
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2022
·Vol. 17
·期 24
·e202200993
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IF 4.839
Zhijie Zhu,Xu Hu,Xingda An,Mengqi Xiao,Liang Zhang,Chaoran Li,Le He
Graphical The influence of the composition of bimetallic nanocrystals on their performance of photothermal catalytic CO 2 hydrogenation was investigated. Pd and Ni play different roles in the photothermal catalytic processes in the bimetallic system, which leads to a functional tradeoff over the stoichiometric ratio. Bimetallic nanomaterials exhibit excellent catalytic performance in photothermal CO 2 hydrogenation due to the synergistic effect between the two metal components. However, the component-performance relationship remains unclear, which hinders the design of efficient bimetallic catalysts and the investigation of catalytic reaction mechanism. Here we illustrate the influence of the composition of binary alloy on their performance of photothermal catalytic CO 2 hydrogenation by using monodispersed Pd−Ni nanocrystal as an example. Our study reveals that Ni and Pd play a significantly different role in the catalytic processes. Higher Ni component in the catalysts could lead to stronger light absorption, higher activity, and lower CO selectivity. The optimized Pd 4 Ni 1 −SiO 2 catalyst exhibited a near-unity and stable CO production rate of 230 mmol ⋅ g −1 ⋅ h −1 under 25-sun illumination. This study paves the way for the usage of bimetal in photothermal CO 2 catalysis towards more efficient solar-to-chemical energy conversions, and sheds light on some general design principles of bimetallic catalysts to balance the intrinsic properties of individual components.
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高影响因子
Gels
·
2022
·Vol. 8
·期 10
·683
·
IF 4.432
Xiangbin Liu,Suling Wang,Weiguang Shi,He Liu
Smart hydrogels, owing to their exceptional viscoelastic and deformable capacity in response to environmental stimulation involving temperature and pH, have been successfully applied in oilfields for purposes such as water and/or gas shutoff treatments. However, the CO2breakthrough problem in low permeability reservoirs has not been well solved. In this work, a rheological method-based Avrami dynamics model and Dickinson dynamics model were employed to investigate the dynamic gelation process of thermo-/pH-dual-sensitive PEG/PAMAM nanogels to further our understanding of the microstructure of their gelation and pertinence plugging application. Plugging experiments were performed by alternating injections of CO2and hydrogel solution in a slug type on three fractured low permeability cores with a backpressure of 13 MPa. The nanogels presented a secondary growth pattern from three to one dimension from micrometer to nanometer size with a morphological transformation from a sphere to an irregular ellipsoid or disk shape. The phase transition temperature was 50 °C, and the phase transition pH was 10. If both or either were below these values, the hydrogel swelled; otherwise, it shrank. Plugging results show that the plugging efficiency was higher than 99%. The maximum breakthrough pressure was 19.93 MPa, and the corresponding residual pressure remained 17.64 MPa for a 10 mD core, exhibiting great plugging performance and high residual resistance after being broken through by CO2.Keywords:smart nanogel;PEG;PAMAM;reaction dynamics;CO2channeling plugging
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CARBON
·
2022
·
IF 11.307
Qingting Zeng,Guangxing Yang,Jianhao Chen,Qiao Zhang,Zhiting Liu,Binhao Qin,Feng Peng
Using carbon black and formamide as raw materials, a N-doped carbon black electrocatalyst (NC) with good performance was prepared by a simple method for the electrochemical CO 2 reduction reaction (ECRR). At −0.86 V vs . RHE , the prepared NC800 catalyst achieves 97.8% of CO selectivity and 9.1 mA cm −2 of CO partial current density, which is higher than most carbon-based electrocatalysts reported so far. In order to better explore the role of nitrogen and oxygen functional groups in carbon-based materials, the nitrogen and oxygen contents in the NC800 catalyst were changed by nitric acid oxidation and thermal desorption. The results show that nitrogen content can effectively improve the CO selectivity of nitrogen-doped carbon materials, but excessive oxygen content inhibits the ECRR activity. It was found for the first time that the ratio of N/(N + O) in carbon catalysts was positively correlated with CO Faraday efficiency and its partial current density, indicating that carbon materials with high nitrogen doping amount and low oxygen content would benefit the ECRR performance, which was also supported by density functional theory calculation. These new understandings provide new insights into the preparation of highly efficient carbon-based catalysts for ECRR.
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